scholarly journals Stratospheric O3 changes during 2001–2010: the small role of solar flux variations in a chemical transport model

2013 ◽  
Vol 13 (19) ◽  
pp. 10113-10123 ◽  
Author(s):  
S. S. Dhomse ◽  
M. P. Chipperfield ◽  
W. Feng ◽  
W. T. Ball ◽  
Y. C. Unruh ◽  
...  

Abstract. Solar spectral fluxes (or irradiance) measured by the SOlar Radiation and Climate Experiment (SORCE) show different variability at ultraviolet (UV) wavelengths compared to other irradiance measurements and models (e.g. NRL-SSI, SATIRE-S). Some modelling studies have suggested that stratospheric/lower mesospheric O3 changes during solar cycle 23 (1996–2008) can only be reproduced if SORCE solar fluxes are used. We have used a 3-D chemical transport model (CTM), forced by meteorology from the European Centre for Medium-Range Weather Forecasts (ECMWF), to simulate middle atmospheric O3 using three different solar flux data sets (SORCE, NRL-SSI and SATIRE-S). Simulated O3 changes are compared with Microwave Limb Sounder (MLS) and Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) satellite data. Modelled O3 anomalies from all solar flux data sets show good agreement with the observations, despite the different flux variations. The off-line CTM reproduces these changes through dynamical information contained in the analyses. A notable feature during this period is a robust positive solar signal in the tropical middle stratosphere, which is due to realistic dynamical changes in our simulations. Ozone changes in the lower mesosphere cannot be used to discriminate between solar flux data sets due to large uncertainties and the short time span of the observations. Overall this study suggests that, in a CTM, the UV variations detected by SORCE are not necessary to reproduce observed stratospheric O3 changes during 2001–2010.

2013 ◽  
Vol 13 (5) ◽  
pp. 12263-12286
Author(s):  
S. S. Dhomse ◽  
M. P. Chipperfield ◽  
W. Feng ◽  
W. T. Ball ◽  
Y. C. Unruh ◽  
...  

Abstract. Solar spectral fluxes (or irradiance) measured by the SOlar Radiation and Climate Experiment (SORCE) show different variability at ultraviolet (UV) wavelengths compared to other irradiance measurements and models (e.g. NRL-SSI, SATIRE-S). Some modelling studies have suggested that stratospheric/lower mesospheric O3 changes during solar cycle 23 (1996–2008) can only be reproduced if SORCE solar fluxes are used. We have used a 3-D chemical transport model (CTM), forced by meteorology from the European Centre for Medium-Range Weather Forecasts (ECMWF), to simulate middle atmospheric O3 using three different solar flux datasets (SORCE, NRL-SSI and SATIRE-S). Simulated O3 changes are compared with Microwave Limb Sounder (MLS) and Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) satellite data. Modelled O3 anomalies from all solar flux datasets show good agreement with the observations, despite the different flux variations. The off-line CTM reproduces these changes through dynamical information contained in the analyses. A notable feature during this period is a robust positive solar signal in the tropical middle stratosphere due to changes in stratospheric dynamics. Ozone changes in the lower mesosphere cannot be used to discriminate between solar flux datasets due to large uncertainties and the short time span of the observations. Overall this study suggests that, in a CTM, the UV variations detected by SORCE are not necessary to reproduce observed stratospheric O3 changes during 2001–2010.


2011 ◽  
Vol 11 (24) ◽  
pp. 12773-12786 ◽  
Author(s):  
S. Dhomse ◽  
M. P. Chipperfield ◽  
W. Feng ◽  
J. D. Haigh

Abstract. We have used an off-line 3-D chemical transport model (CTM) to investigate the 11-yr solar cycle response in tropical stratospheric ozone. The model is forced with European Centre for Medium-Range Weather Forecasts (ECMWF) (re)analysis (ERA-40/operational and ERA-Interim) data for the 1979–2005 time period. We have compared the modelled solar response in ozone to observation-based data sets that are constructed using satellite instruments such as Total Ozone Mapping Spectrometer (TOMS), Solar Backscatter UltraViolet instrument (SBUV), Stratospheric Aerosol and Gas Experiment (SAGE) and Halogen Occultation Experiment (HALOE). A significant difference is seen between simulated and observed ozone during the 1980s, which is probably due to inhomogeneities in the ERA-40 reanalyses. In general, the model with ERA-Interim dynamics shows better agreement with the observations from 1990 onwards than with ERA-40. Overall both standard model simulations are partially able to simulate a "double peak"-structured ozone solar response with a minimum around 30 km, and these are in better agreement with HALOE than SAGE-corrected SBUV (SBUV/SAGE) or SAGE-based data sets. In the tropical lower stratosphere (TLS), the modelled solar response with time-varying aerosols is amplified through aliasing with a volcanic signal, as the model overestimates ozone loss during high aerosol loading years. However, the modelled solar response with fixed dynamics and constant aerosols shows a positive signal which is in better agreement with SBUV/SAGE and SAGE-based data sets in the TLS. Our model simulations suggests that photochemistry contributes to the ozone solar response in this region. The largest model-observation differences occur in the upper stratosphere where SBUV/SAGE and SAGE-based data show a significant (up to 4%) solar response whereas the standard model and HALOE do not. This is partly due to a positive solar response in the ECMWF upper stratospheric temperatures which reduces the modelled ozone signal. The large positive upper stratospheric solar response seen in SBUV/SAGE and SAGE-based data can be reproduced in model runs with fixed dynamical fields (i.e. no inter-annual meteorological changes). As these runs effectively assume no long-term temperature changes (solar-induced or otherwise), it should provide an upper limit of the ozone solar response. Overall, full quantification of the solar response in stratospheric ozone is limited by differences in the observed data sets and by uncertainties in the solar response in stratospheric temperatures.


2021 ◽  
Vol 13 (12) ◽  
pp. 5711-5729
Author(s):  
Sandip S. Dhomse ◽  
Carlo Arosio ◽  
Wuhu Feng ◽  
Alexei Rozanov ◽  
Mark Weber ◽  
...  

Abstract. High-quality stratospheric ozone profile data sets are a key requirement for accurate quantification and attribution of long-term ozone changes. Satellite instruments provide stratospheric ozone profile measurements over typical mission durations of 5–15 years. Various methodologies have then been applied to merge and homogenise the different satellite data in order to create long-term observation-based ozone profile data sets with minimal data gaps. However, individual satellite instruments use different measurement methods, sampling patterns and retrieval algorithms which complicate the merging of these different data sets. In contrast, atmospheric chemical models can produce chemically consistent long-term ozone simulations based on specified changes in external forcings, but they are subject to the deficiencies associated with incomplete understanding of complex atmospheric processes and uncertain photochemical parameters. Here, we use chemically self-consistent output from the TOMCAT 3-D chemical transport model (CTM) and a random-forest (RF) ensemble learning method to create a merged 42-year (1979–2020) stratospheric ozone profile data set (ML-TOMCAT V1.0). The underlying CTM simulation was forced by meteorological reanalyses, specified trends in long-lived source gases, solar flux and aerosol variations. The RF is trained using the Stratospheric Water and OzOne Satellite Homogenized (SWOOSH) data set over the time periods of the Microwave Limb Sounder (MLS) from the Upper Atmosphere Research Satellite (UARS) (1991–1998) and Aura (2005–2016) missions. We find that ML-TOMCAT shows excellent agreement with available independent satellite-based data sets which use pressure as a vertical coordinate (e.g. GOZCARDS, SWOOSH for non-MLS periods) but weaker agreement with the data sets which are altitude-based (e.g. SAGE-CCI-OMPS, SCIAMACHY-OMPS). We find that at almost all stratospheric levels ML-TOMCAT ozone concentrations are well within uncertainties of the observational data sets. The ML-TOMCAT (V1.0) data set is ideally suited for the evaluation of chemical model ozone profiles from the tropopause to 0.1 hPa and is freely available via https://doi.org/10.5281/zenodo.5651194 (Dhomse et al., 2021).


2011 ◽  
Vol 11 (5) ◽  
pp. 13975-14001 ◽  
Author(s):  
S. Dhomse ◽  
M. P. Chipperfield ◽  
W. Feng ◽  
J. D. Haigh

Abstract. We have used an off-line 3-D chemical transport model (CTM), to investigate the 11-year solar cycle response in tropical stratospheric ozone. The model is forced with European Centre for Medium-Range Weather Forecasts (ECMWF) (re)analysis (ERA-40/Operational and ERA-Interim) data for 1978–2005 time period. We have compared the modelled solar response in ozone to observational data from three satellite instruments, Solar Backscatter UltraViolet instrument (SBUV), Stratospheric Aerosol and Gas Experiment (SAGE) and Halogen Occultation Experiment (HALOE). A significant difference is seen between simulated and observed ozone during the 1980s, which is probably due to inhomogeneities in the ERA-40 reanalyses. In general, the model with ERA-Interim dynamics shows better agreement with the observations from 1990 onwards than ERA-40. Overall both standard model simulations are partially able to simulate a "double peak"-structured ozone solar response profile with a minimum around 30 km, and these are in better agreement with HALOE than SBUV or SAGE. The largest model-observation differences occur in the upper stratosphere where SBUV and SAGE show a significant (up to 4 %) solar response whereas the standard model and HALOE do not. This is partly due to a positive solar response in the ECMWF upper stratosphere analysed temperatures which reduces the modelled ozone signal. The large positive upper stratosphere response seen in SAGE/SBUV can be reproduced in a model run with fixed dynamical fields (i.e. no inter-annual meteorological changes). As this run effectively assumes no long-term temperature changes (solar-induced or otherwise) it should provide an upper limit of the ozone solar response. Overall, full quantification of the upper stratosphere ozone solar response is limited by differences in the observed dataset and by uncertainties in the solar response in the stratospheric temperatures. In the lower stratosphere we find that transport by analysed winds, which contain information about the Quasi-Biennial Oscillation (QBO), can lead to a large ozone solar response. However, the run with fixed dynamical fields also produces a positive solar response (up to 2 %) in line with the SAGE and SBUV observations.


2012 ◽  
Vol 12 (16) ◽  
pp. 7825-7865 ◽  
Author(s):  
D. Simpson ◽  
A. Benedictow ◽  
H. Berge ◽  
R. Bergström ◽  
L. D. Emberson ◽  
...  

Abstract. The Meteorological Synthesizing Centre-West (MSC-W) of the European Monitoring and Evaluation Programme (EMEP) has been performing model calculations in support of the Convention on Long Range Transboundary Air Pollution (CLRTAP) for more than 30 years. The EMEP MSC-W chemical transport model is still one of the key tools within European air pollution policy assessments. Traditionally, the model has covered all of Europe with a resolution of about 50 km × 50 km, and extending vertically from ground level to the tropopause (100 hPa). The model has changed extensively over the last ten years, however, with flexible processing of chemical schemes, meteorological inputs, and with nesting capability: the code is now applied on scales ranging from local (ca. 5 km grid size) to global (with 1 degree resolution). The model is used to simulate photo-oxidants and both inorganic and organic aerosols. In 2008 the EMEP model was released for the first time as public domain code, along with all required input data for model runs for one year. The second release of the EMEP MSC-W model became available in mid 2011, and a new release is targeted for summer 2012. This publication is intended to document this third release of the EMEP MSC-W model. The model formulations are given, along with details of input data-sets which are used, and a brief background on some of the choices made in the formulation is presented. The model code itself is available at www.emep.int, along with the data required to run for a full year over Europe.


2015 ◽  
Vol 15 (2) ◽  
pp. 829-843 ◽  
Author(s):  
T. Sakazaki ◽  
M. Shiotani ◽  
M. Suzuki ◽  
D. Kinnison ◽  
J. M. Zawodny ◽  
...  

Abstract. This paper contains a comprehensive investigation of the sunset–sunrise difference (SSD, i.e., the sunset-minus-sunrise value) of the ozone mixing ratio in the latitude range of 10° S–10° N. SSD values were determined from solar occultation measurements based on data obtained from the Stratospheric Aerosol and Gas Experiment (SAGE) II, the Halogen Occultation Experiment (HALOE), and the Atmospheric Chemistry Experiment–Fourier transform spectrometer (ACE–FTS). The SSD was negative at altitudes of 20–30 km (−0.1 ppmv at 25 km) and positive at 30–50 km (+0.2 ppmv at 40–45 km) for HALOE and ACE–FTS data. SAGE II data also showed a qualitatively similar result, although the SSD in the upper stratosphere was 2 times larger than those derived from the other data sets. On the basis of an analysis of data from the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) and a nudged chemical transport model (the specified dynamics version of the Whole Atmosphere Community Climate Model: SD–WACCM), we conclude that the SSD can be explained by diurnal variations in the ozone concentration, particularly those caused by vertical transport by the atmospheric tidal winds. All data sets showed significant seasonal variations in the SSD; the SSD in the upper stratosphere is greatest from December through February, while that in the lower stratosphere reaches a maximum twice: during the periods March–April and September–October. Based on an analysis of SD–WACCM results, we found that these seasonal variations follow those associated with the tidal vertical winds.


1999 ◽  
Vol 104 (D9) ◽  
pp. 11755-11781 ◽  
Author(s):  
Eugene V. Rozanov ◽  
Vladimir A. Zubov ◽  
Michael E. Schlesinger ◽  
Fanglin Yang ◽  
Natalia G. Andronova

2012 ◽  
Vol 12 (15) ◽  
pp. 7073-7085 ◽  
Author(s):  
J. Kuttippurath ◽  
S. Godin-Beekmann ◽  
F. Lefèvre ◽  
G. Nikulin ◽  
M. L. Santee ◽  
...  

Abstract. We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period of time, from December to mid-April, and a strong and stable vortex was present during that period. Simulations with the Mimosa-Chim CTM show that the chemical ozone loss started in early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh−1 (parts per billion by volume/sunlit hour) and a contribution of about 30–55% and 30–35% from the ClO-ClO and ClO-BrO cycles, respectively, in late February and March. In addition, a contribution of 30–50% from the HOx cycle is also estimated in April. We also estimate a loss of about 0.7–1.2 ppmv contributed (75%) by the NOx cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements.


2016 ◽  
Vol 9 (8) ◽  
pp. 2741-2754 ◽  
Author(s):  
Elham Baranizadeh ◽  
Benjamin N. Murphy ◽  
Jan Julin ◽  
Saeed Falahat ◽  
Carly L. Reddington ◽  
...  

Abstract. The particle formation scheme within PMCAMx-UF, a three-dimensional chemical transport model, was updated with particle formation rates for the ternary H2SO4–NH3–H2O pathway simulated by the Atmospheric Cluster Dynamics Code (ACDC) using quantum chemical input data. The model was applied over Europe for May 2008, during which the EUCAARI-LONGREX (European Aerosol Cloud Climate and Air Quality Interactions–Long-Range Experiment) campaign was carried out, providing aircraft vertical profiles of aerosol number concentrations. The updated model reproduces the observed number concentrations of particles larger than 4 nm within 1 order of magnitude throughout the atmospheric column. This agreement is encouraging considering the fact that no semi-empirical fitting was needed to obtain realistic particle formation rates. The cloud adjustment scheme for modifying the photolysis rate profiles within PMCAMx-UF was also updated with the TUV (Tropospheric Ultraviolet and Visible) radiative-transfer model. Results show that, although the effect of the new cloud adjustment scheme on total number concentrations is small, enhanced new-particle formation is predicted near cloudy regions. This is due to the enhanced radiation above and in the vicinity of the clouds, which in turn leads to higher production of sulfuric acid. The sensitivity of the results to including emissions from natural sources is also discussed.


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